Low-Temperature Single Carbon Nanotube Spectroscopy of sp3 Quantum Defects

He, Xiaowei; Gifford, Brendan Joel; Hartmann, Nicolai; Ihly, Rachelle; Ma, Xuedan; Kilina, Svetlana V.; Luo, Yue; Shayan, Kamarn; Strauf, Stefan; Blackburn, Jeffrey; Tretiak, Sergei; Doorn, Stephen K.; Htoon, Han

doi:10.1021/acsnano.7b03022

Title: Low-Temperature Single Carbon Nanotube Spectroscopy of sp³ Quantum Defects

Journal Article · Thu Sep 28 00:00:00 EDT 2017 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.7b03022· OSTI ID:1477667

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Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division and Center for Nonlinear Studies; North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
National Renewable Energy Lab. (NREL), Golden, CO (United States). National Center for Photovoltaics. Chemical and Materials Science Center
North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
Stevens Inst. of Technology, Hoboken, NJ (United States). Dept. of Physics
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies, Theoretical Division and Center for Nonlinear Studies

Aiming to unravel the relationship between chemical configuration and electronic structure of sp3 defects of aryl-functionalized (6,5) single-walled carbon nanotubes (SWCNTs), we perform low-temperature single nanotube photoluminescence (PL) spectroscopy studies and correlate our observations with quantum chemistry simulations. Here, we observe sharp emission peaks from individual defect sites that are spread over an extremely broad, 1000-1350 nm, spectral range. Our simulations allow us to attribute this spectral diversity to the occurrence of six chemically and energetically distinct defect states resulting from topological variation in the chemical binding configuration of the monovalent aryl groups. Both PL emission efficiency and spectral line width of the defect states are strongly influenced by the local dielectric environment. Wrapping the SWCNT with a polyfluorene polymer provides the best isolation from the environment and yields the brightest emission with near-resolution limited spectral line width of 270 ueV, as well as spectrally resolved emission wings associated with localized acoustic phonons. Pump-dependent studies further revealed that the defect states are capable of emitting single, sharp, isolated PL peaks over 3 orders of magnitude increase in pump power, a key characteristic of two-level systems and an important prerequisite for single-photon emission with high purity. Our findings point to the tremendous potential of sp3 defects in development of room temperature quantum light sources capable of operating at telecommunication wavelengths as the emission of the defect states can readily be extended to this range via use of larger diameter SWCNTs.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC52-06NA25396; AC36-08GO28308; AC02-05CH11231; DMR-1506711; ECCS-MRI-1531237; CHE-1413614

OSTI ID:: 1477667

Alternate ID(s):: OSTI ID: 1400371

Report Number(s):: LA-UR-18-25425; NREL/JA-5900-70314

Journal Information:: ACS Nano, Vol. 11, Issue 11; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 59 works

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carbon nanotubes
diazonium doping
electronic structure
exciton localization
photoluminescence

Title: Low-Temperature Single Carbon Nanotube Spectroscopy of sp3 Quantum Defects

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Title: Low-Temperature Single Carbon Nanotube Spectroscopy of sp³ Quantum Defects